你好,
使用Margin, VerticalAlignment属性就可以。
<Grid x:Name="LayoutRoot" Background="Gray">
<Button x:Name="btn" Background="Red" VerticalAlignment="Top" HorizontalAlignment="Left" Margin="0,0,0,0" Content="button" Foreground="Brown" Height="80" Width="200" />
</Grid>
Button的样式里内嵌的Grid默认是透明的(Background="
Transparent"),可能你看到的没有对齐,是由于这个而导致的视觉效果,将Grid的Background属性改成其他颜色就可以看出来了。如图所示:

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